Efficient Visible-Light-Driven Carbon Dioxide Reduction by a Single-Atom Implanted Metal-Organic Framework

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• 作者：Dr. Huabin Zhang ; Dr. Jing Wei ; Dr. Juncai Dong ; Dr. Guigao Liu ; Li Shi ; Dr. Pengfei An ; Dr. Guixia Zhao ; Dr. Jintao Kong ; Dr. Xiaojun Wang ; Dr. Xianguang Meng ; Prof. Jing Zhang and Prof. Jinhua Ye
• 刊名：Angewandte Chemie
• 出版年：2016
• 出版时间：November 7, 2016
• 年：2016
• 卷：128
• 期：46
• 页码：14522-14526
• 全文大小：2267K
• ISSN：1521-3757

文摘

Modular optimization of metal–organic frameworks (MOFs) was realized by incorporation of coordinatively unsaturated single atoms in a MOF matrix. The newly developed MOF can selectively capture and photoreduce CO₂ with high efficiency under visible-light irradiation. Mechanistic investigation reveals that the presence of single Co atoms in the MOF can greatly boost the electron–hole separation efficiency in porphyrin units. Directional migration of photogenerated excitons from porphyrin to catalytic Co centers was witnessed, thereby achieving supply of long-lived electrons for the reduction of CO₂ molecules adsorbed on Co centers. As a direct result, porphyrin MOF comprising atomically dispersed catalytic centers exhibits significantly enhanced photocatalytic conversion of CO₂, which is equivalent to a 3.13-fold improvement in CO evolution rate (200.6 μmol g⁻¹ h⁻¹) and a 5.93-fold enhancement in CH₄ generation rate (36.67 μmol g⁻¹ h⁻¹) compared to the parent MOF.